The discovery of room-temperature single photon emission from color centers in diamond has in recent years boosted research interest in this renowned material in photonics and quantum community and beyond. Following understanding some basic principles of how the color centers work, new challenges arose: designing and fabricating real devices that leverage the unrivaled properties that diamond possesses. Due to this material's extreme physical hardness and its chemical resistance to etchants, the established semiconductor technologies cannot straightforwardly answer to the call for scalable and reliable fabrication of micro- and nano-photonic devices in single crystal diamond. In this thesis, we first demonstrate an unconventional polishing protocol with ion beam etching, which makes possible wafer-scale fine finishing of diamond substrates, the starting point for any subsequent processing. Following this we present the experimental observation of self-organized nanotextures on diamond induced by ion beam irradiation, a lithography-free approach for nanoengineering periodic structures. Regarding device fabrication, we obtained free-standing micro- and nano-photonic structures using angled reactive ion etching, facilitated by a novel and reproducible Faraday cage design. We also propose possible designs to interconnect individual components in hope of realizing a photonic integrated circuit in the future. Last but not least, we present spectroscopic characterization of single and ensemble color centers either grown by microwave plasma chemical vapor deposition, or fabricated by ion implantation with subsequent high-temperature annealing, which are the fundamental building blocks for quantum applications. Photoluminescence spectra that, to our knowledge, are not seen in literature were recorded for ensemble silicon-vacancy centers at cryogenic temperature, signifying potentially unknown mechanism for tuning the optical transitions, and unexplored possibilities with this exciting material platform for quantum technologies.
The discovery of room-temperature single photon emission from color centers in diamond has in recent years boosted research interest in this renowned material in photonics and quantum community and beyond. Following understanding some basic principles of how the color centers work, new challenges arose: designing and fabricating real devices that leverage the unrivaled properties that diamond possesses. Due to this material's extreme physical hardness and its chemical resistance to etchants, the established semiconductor technologies cannot straightforwardly answer to the call for scalable and reliable fabrication of micro- and nano-photonic devices in single crystal diamond. In this thesis, we first demonstrate an unconventional polishing protocol with ion beam etching, which makes possible wafer-scale fine finishing of diamond substrates, the starting point for any subsequent processing. Following this we present the experimental observation of self-organized nanotextures on diamond induced by ion beam irradiation, a lithography-free approach for nanoengineering periodic structures. Regarding device fabrication, we obtained free-standing micro- and nano-photonic structures using angled reactive ion etching, facilitated by a novel and reproducible Faraday cage design. We also propose possible designs to interconnect individual components in hope of realizing a photonic integrated circuit in the future. Last but not least, we present spectroscopic characterization of single and ensemble color centers either grown by microwave plasma chemical vapor deposition, or fabricated by ion implantation with subsequent high-temperature annealing, which are the fundamental building blocks for quantum applications. Photoluminescence spectra that, to our knowledge, are not seen in literature were recorded for ensemble silicon-vacancy centers at cryogenic temperature, signifying potentially unknown mechanism for tuning the optical transitions, and unexplored possibilities with this exciting material platform for quantum technologies.
Recently, developments in novel and high-purity materials allow for the presence of a single, solitary crystalline defect to define the electronic, magnetic, and optical functionality of a device. The discrete nature of the active dopant, whose properties are defined by a quantum mechanical description of its structure, enables radically new quantum investigations and applications in these arenas. Finally,there has been significant development in large-scale device engineering due to mature semiconductor manufacturing techniques. The diverse set of photonic device architectures offering light confinement, guiding, and extraction is a prime example. These three paradigms – solitary dopant photonics and optoelectronics (solotronics), quantum science\tand technology, and device engineering – merge in the development of novel quantum photonic devices for the next generation of information processing systems. We present in this thesis a series of investigations of optical nanostructures for single optically active spins in single crystal diamond. Chapter 1 introduces the Nitrogen-Vacancy (NV) color center, summarizes its applications, and motivates the need for their integration into photonic structures. Chapter 2 describes two prototype nanobeam photonic crystal cavities for generating strong light-matter interactions with NV centers. The first device consists of a silicon nitride photonic crystal nanobeam cavity with high quality factor \\(Q \\sim 10^5\\) and small mode volume \\(V \\sim 0.5*(\\lambda/n)^3\\). The second device consists of a monolithic diamond nanobeam cavity fabricated with the focused ion beam (FIB) directly in a single crystal diamond sample. Chapter 3 presents a high-efficiency source of single photons consisting of a single NV center in a photonic diamond nanowire. Early FIB prototypes are described, as is the first successful realization of the device achieved via reactive ion etching nanowires in a single crystal diamond containing NV centers, and finally a variation of this approach based on incorporation of NV centers in pure diamond via ion implantation. In chapter 4 we consider the optimal design of photonic devices offering both collection efficiency and cavity-enhancements and extend the model of the NV center to include photonic effects. In chapter 5 we briefly introduce a novel optically active spin discovered in a diamond nanowire. Finally, in chapter 6 we conclude with several proposals to extend this research program.
Luminescent lattice defects (so called “color centers”) in diamond provide a robust, solid-state architecture for exploring quantum optics, with many facilitating direct access to highly coherent electron and nuclear spins. The past two decades have seen tremendous advances in our ability to prepare and control the quantum states of these atom-like systems. For instance, demonstrations that leverage the diamond nitrogen vacancy (NV–) center as a spin-photon interface have included the generation of indistinguishable photons, a quantum bit memory exceeding 1 second, entanglement of two distance solid-state qubits, and deterministic long distance quantum teleportation. While diamond color centers are an attractive platform for scalable quantum information processing, the diamond solid-state matrix, by its very nature, inhibits efficient photon collection into either free-space or fiber-optical systems. Due to its large refractive index, emitted photons are inevitably trapped within the diamond crystal by total internal reflection, limiting count rates and overall scalability of information processing via quantum optical protocols. To this end, there has been significant progress towards integrating individual diamond color centers within well-defined radiation channels: namely, those provided by monolithic diamond nanophotonic networks. Currently, on-chip low loss (~ few db/cm) diamond waveguide networks are available, as well as key passive photonic elements like micron scale ring and disk resonators and photonic crystal cavities, with high optical quality (Q) factors. Specifically, we recently demonstrated a scalable ‘angled-etching’ nanofabrication method for realizing nanophotonic networks starting from bulk single-crystal diamond substrates (MJ Burek et al., Nano Letters 2012, MJ Burek et al., Nat Comm. 2014). Angled-etching employs anisotropic oxygen-based plasma etching at an oblique angle to the substrate surface, resulting in suspended optical structures with triangular cross-sections. Using this approach, we demonstrated high Q-factor (> 10^5) optical nanocavities fabricated in bulk single-crystal diamond, operating over a wide wavelength range (visible to telecom). Beyond isolated photonic devices, we have further developed free-standing angled-etched waveguides which efficiently route photons between diamond optical nanocavities, while maintaining physical support through attachment to the bulk substrate. Although on-chip diamond nanophotonics realized by angled-etching continue to mature, efficient off-chip optical coupling schemes which provide near seamless transition of photons on-chip into commercial optical fibers remain an outstanding challenge. This is especially pertinent in applications involving single photons, such as quantum optics with diamond color centers. Herein, we demonstrate a high efficiency fiber-optical interface with aforementioned on-chip diamond nanophotonic networks, achieving > 90% power coupling at both telecom and visible wavelengths. The coupling scheme utilizes a single mode optical fiber, with one end fabricated into a conical taper, to adiabatically transition guided light between on-chip tapered diamond waveguides and off-chip optical fiber networks. Additionally, we develop techniques to robustly pigtail single-mode fibers with diamond waveguide couplers, yielding a packaged technology that may potentially enable deployment in harsh environments, including vacuum, sub-Kelvin cryogenics, or even liquid/biological environments. With these newly developed optical integration schemes, single-crystal diamond is now a viable integrated nanophotonics platform, servicing a range of applications, from non-linear optics and chemical sensing, to quantum science and cavity optomechanics.
We demonstrate the coupling of single color centers in diamond to plasmonic and dielectric photonic structures to realize novel nanophotonic devices. Nanometer spatial control in the creation of single color centers in diamond is achieved by implantation of nitrogen atoms through high-aspect-ratio channels in a mica mask. Enhanced broadband single-photon emission is demonstrated by coupling nitrogen-vacancy centers to plasmonic resonators, such as metallic nanoantennas. Improved photon-collection efficiency and directed emission is demonstrated by solid immersion lenses and micropillar cavities. Thereafter, the coupling of diamond nanocrystals to the guided modes of micropillar resonators is discussed along with experimental results. Finally, we present a gas-phase-doping approach to incorporate color centers based on nickel and tungsten, in situ into diamond using microwave-plasma-enhanced chemical vapor deposition. The fabrication of silicon-vacancy centers in nanodiamonds by microwave-plasma-enhanced chemical vapor deposition is discussed in addition.
Quantum communication and quantum metrology established a demand for an accessible solid state systems which can generate a stream of single photons on demand [1]. Although single photon emission has been demonstrated from quantum dots (QD)[1,2], single molecules [3] and nanowires [4], their practical operation is limited by the temperature or photostability. Diamond crystals, however, are the most promising platform for generation of robust, photo-stable, single photons at room temperature [5,6]. Nevertheless, out of more than 500 existing optical centers in diamond only three known centers demonstrated a clear single photon emission: the nitrogen-vacancy complex [6,7], the silicon-vacancy complex [8] and the nickel-nitrogen complex [9,10]. Recent progress in materials science and fabrication techniques of diamond color centers unveiled novel quantum emitters with photo-physical properties surpassing the current mainstream [11,12,13]. Consequently, the versatility of the diamond lattice to host various impurities which give luminescence signals lead to a dramatic discovery of ultra bright single photon emitters operating in the MHz regime [14]. These new centers, comparable with QD in terms of brightness [1], but have the tremendous advantage of their room temperature operation and photo-stability. Furthermore, it opened a new avenue to investigate essentially an unknown group of single photon emitters. A brief description of the fabrication methods and a detailed quantum optical characterization of this class of diamond emitters is the subject of this presentation. In particular we will present the photo-physical properties of a novel family of single photon emitters, most likely originated from Cr impurities within the chemical vapor deposition grown nano-diamond crystals. We concentrate on the typical emission lines in the range of 740 - 790 nm, which exhibit single photon emission with count rate in the range of 0.8-3.2 106 counts/s at the limit of infinite optical excitation power, and life time as short as 1 ns. Even more, some of the emitters exhibit a photon statistics without any photon bunching, indicating a two-level system with unitary quantum efficiency. We will also show preliminary results of a resonant excitation at 4 K. We will highlight future directions to optimize these sources and avenues to investigate the fundamental properties of these centers.
Silicon-vacancy (SiV) centers in diamond are gaining an increased interest for application, such as in quantum technologies and sensing. Due to the strong luminescence concentrated in its sharp zero-phonon line at room temperature, SiV centers are being investigated as single-photon sources for quantum communication, and also as temperature probes for sensing. Here, we discussed strategies for the fabrication of SiV centers in diamond based on Si-ion implantation followed by thermal activation. SiV color centers in high-quality single crystals have the best optical properties, but polycrystalline micro and nanostructures are interesting for applications in nano-optics. Moreover, we discuss the photoluminescence properties of SiV centers in phosphorous-doped diamond, which are relevant for the creation of electroluminescent devices, and nanophotonics strategies to improve the emission characteristics of the SiV centers. Finally, the optical properties of such centers at room and high temperatures show the robustness of the center and give perspectives for temperature-sensing applications.
Efficient interfaces between optical photons and quantum bits are fundamental building blocks for quantum networks and large-scale quantum computers. We demonstrate an integrated platform for scalable quantum optics based on color centers coupled to diamond nanodevices. First, we incorporate nitrogen-vacancy (NV) centers in diamond into hybrid nanophotonic crystal cavities. Despite our progress towards coupling the NV to cavity photons, we find that the NV-cavity interface is limited by the imperfections of the color center's properties and its local environment. We approach this challenge first by characterizing and modifying the diamond surface to reduce the environmental noise affecting the NV optical transition. Subsequently, we develop a new approach that makes use of a quantum emitter with intrinsic protection from this noise: the silicon-vacancy (SiV) center in diamond. We demonstrate that SiV centers introduced through ion implantation feature highly coherent optical transitions, even inside nanostructures. By placing SiV centers inside all-diamond photonic crystal cavities, we achieve strong SiV-photon coupling with a cooperativity of greater than 20. Using this platform, we realize a quantum-optical switch controlled by the spin degree of freedom of a single SiV. By measuring intensity correlations of indistinguishable Raman photons emitted into a single waveguide, we observe a quantum interference effect resulting from the superradiant emission of two probabilistically entangled SiV centers. Finally, we demonstrate controllable photon-mediated interactions between the spin degrees of freedom of two cavity-coupled SiV centers. When the optical transitions of the two SiV centers are tuned into resonance, the coupling of each SiV to the common cavity mode results in a coherent interaction between the two SiVs, leading to the observation of super- and sub-radiant two-SiV states.